The invention includes: a new composition of matter (a composite comprising a naturally occurring in vivo cornea in an in situ eye together with at least one volume of vitrified non-naturally occurring corneal stromal tissue formed within the naturally occurring corneal stromal tissue) wherein the vitrified tissue is modified in structure and properties from its naturally occurring condition into a non-naturally occurring glass-like condition with modifications including but not limited to increased elastic modulus; methods for producing and using the new composition of matter for modifying corneal structure and properties, including but not limited to corneal optical aberrations; wound closure adhesion and transplant adhesion; and a photovitrification system for producing the new composition of matter comprising at least one photon source with controllable treatment parameters. A reverse template can be added to corneal vitrification systems to increase vitrification and modifications of structure and properties.